Separation technologies are key for the chemical processing of the massive amount of polycotton waste generated worldwide. The distinct chemical nature of cellulose and polyethylene terephthalate (PET) guides the design of fractionation strategies to obtain two valuable monomaterial streams. The optimal fractionation process is, in our view, highly context dependent what conveys to seek a variety of alternatives seeking for chemical processes driven by the ulterior up-cycling of the monomaterial streams. On the PET side, alkaline depolymerization yields monomers for the synthesis of recycled polyester, while cellulose remains as fiber-grade feedstock. Alternatively, we investigate pathways that chemically transform the cellulose fraction into spinnable mixtures or fermentable sugars for further valorisation. This research supports the development of chemical routes for the recycling of mixed textile waste.